Aqueous Li-ion battery enabled by halogen conversion-intercalation chemistry in graphite

被引:674
作者
Yang, Chongyin [1 ]
Chen, Ji [1 ]
Ji, Xiao [1 ]
Pollard, Travis P. [2 ]
Lu, Xujie [3 ]
Sun, Cheng-Jun [4 ]
Hou, Singyuk [1 ]
Liu, Qi [4 ,5 ]
Liu, Cunming [4 ]
Qing, Tingting [1 ]
Wang, Yingqi [3 ]
Borodin, Oleg [2 ]
Ren, Yang [4 ]
Xu, Kang [2 ]
Wang, Chunsheng [1 ,6 ]
机构
[1] Univ Maryland, Dept Chem & Biomol Engn, College Pk, MD 20742 USA
[2] US Army, Electrochem Branch, Power & Energy Div, Sensor & Electron Devices Directorate,Res Lab, Adelphi, MD USA
[3] Ctr High Pressure Sci & Technol Adv Res, Shanghai, Peoples R China
[4] Argonne Natl Lab, Adv Photon Source, Xray Sci Div, Argonne, IL 60439 USA
[5] City Univ Hong Kong, Dept Phys, Hong Kong, Peoples R China
[6] Univ Maryland, Dept Chem & Biochem, College Pk, MD 20742 USA
关键词
GENERALIZED GRADIENT APPROXIMATION; MOLECULAR-DYNAMICS SIMULATIONS; POLARIZABLE FORCE-FIELD; ELECTROCHEMICAL INTERCALATION; CRYSTAL-STRUCTURE; BROMINE; LITHIUM; TRANSPORT; EXAFS; OXIDE;
D O I
10.1038/s41586-019-1175-6
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
The use of 'water-in-salt' electrolytes has considerably expanded the electrochemical window of aqueous lithium-ion batteries to 3 to 4 volts, making it possible to couple high-voltage cathodes with low-potential graphite anodes(1-4). However, the limited lithium intercalation capacities (less than 200 milliampere-hours per gram) of typical transition-metal-oxide cathodes(5,6) preclude higher energy densities. Partial(7,8) or exclusive(9) anionic redox reactions may achieve higher capacity, but at the expense of reversibility. Here we report a halogen conversion-intercalation chemistry in graphite that produces composite electrodes with a capacity of 243 milliampere-hours per gram (for the total weight of the electrode) at an average potential of 4.2 volts versus Li/Li+. Experimental characterization and modelling attribute this high specific capacity to a densely packed stage-I graphite intercalation compound, C-3.5[Br0.5Cl0.5], which can form reversibly in water-in-bisalt electrolyte. By coupling this cathode with a passivated graphite anode, we create a 4-volt-class aqueous Li-ion full cell with an energy density of 460 watt-hours per kilogram of total composite electrode and about 100 per cent Coulombic efficiency. This anion conversion-intercalation mechanism combines the high energy densities of the conversion reactions, the excellent reversibility of the intercalation mechanism and the improved safety of aqueous batteries.
引用
收藏
页码:245 / +
页数:19
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